Time-resolved photoelectron spectroscopy of IR-driven electron dynamics in a charge transfer model system

Falge, Mirjam; Fröbel, Friedrich Georg; Engel, Volker; Gräfe, Stefanie

doi:10.1039/c7cp01832k

Cited by 5 publications

(9 citation statements)

References 37 publications

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“…We attribute this to the chosen near-equilibrium initial conditions for χ(R). Previous studies have shown, that nuclear dynamics following initial non-equilibrium configurations is reflected in the photoelectron momentum distribution [37,38]. Investigations of such effects on the correlation-driven knock-up and knockdown processes are currently under way in our workgroup.…”

Section: Restricted Electron-field Interactionsmentioning

confidence: 90%

“…where R e scales the electron-electron interaction [34][35][36][37][38][39][40]. The fixed nuclei have a distance of L = 10 Å.…”

Section: Theorymentioning

confidence: 99%

“…Nuclear charges are Z = Z 1 = Z 2 = 1. All truncation parameters have been set to R f = R c = R e = 1.5 Å, corresponding to the weak-coupling regime [38]. The three particle configuration of the model and its dynamics can be fully solved numerically.…”

Section: Theorymentioning

confidence: 99%

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The impact of electron–electron correlation in ultrafast attosecond single ionization dynamics

Fröbel

Ziems

Peschel

et al. 2020

J. Phys. B: At. Mol. Opt. Phys.

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The attosecond ultrafast ionization dynamics of correlated two-or many-electron systems have, so far, been mainly addressed investigating atomic systems. In the case of single ionization, it is well known that electronelectron correlation modifies the ionization dynamics and observables beyond the single active electron picture, resulting in effects such as the Auger effect or shake-up/down and knock-up/down processes. Here, we extend these works by investigating the attosecond ionization of a molecular system involving correlated two-electron dynamics, as well as non-adiabatic nuclear dynamics. Employing a charge-transfer molecular model system with two differently bound electrons, a strongly and a weakly bound electron, we distinguish different pathways leading to ionization, be it direct ionization or ionization involving elastic and inelastic electron scattering processes. We find that different pathways result in a difference in the electronic population of the parent molecular ion, which, in turn, involves different subsequent (non-adiabatic) postionization dynamics on different time scales.

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Section: Restricted Electron-field Interactionsmentioning

confidence: 90%

“…where R e scales the electron-electron interaction [34][35][36][37][38][39][40]. The fixed nuclei have a distance of L = 10 Å.…”

Section: Theorymentioning

confidence: 99%

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The impact of electron–electron correlation in ultrafast attosecond single ionization dynamics

Fröbel

Ziems

Peschel

et al. 2020

J. Phys. B: At. Mol. Opt. Phys.

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“…This type of potential was originally introduced by Sprik et al [36] and extensively used by H. Metiu [32,37], V. Engel [33,38] and S. Gräfe [34,39] to study coupled electron-nuclear dynamics in molecular systems. By choice of z = 0.9048 for the effective nuclear charge and a = 1.8544 Å for the screening parameter, the model reproduces the ionization potential (IP) ε ip = 5.139 eV of sodium and the prominent 3p → 3s sodium D-line at λ D = 589 nm, i.e.…”

Section: A Theoretical Descriptionmentioning

confidence: 99%

Atomic photoionization dynamics in ultrashort cycloidal laser fields

Bayer,

Philipp,

Eickhoff

et al. 2020

Preprint

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We present numerical simulations of ultrafast multiphoton ionization dynamics in a twodimensional atomic model driven by co-and counterrotating circularly polarized single-color and bichromatic carrier envelope phase (CEP) stable ultrashort laser pulse sequences. Taking into account phase variations due to CEP fluctuations and the Gouy phase, our results accurately reproduce recently measured photoelectron momentum distributions [1][2][3][4]. The time evolution of the complexvalued electron wave function in coordinate and momentum space is calculated to study the bound state-and the vortex formation dynamics. The non-vanishing azimuthal probability current density proves the vortex nature of electron wave packets with odd-numbered rotational symmetry. Their angular momentum expectation value assumes half-integer values of 3.5 (corotating) and 0.5 (counterrotating). Knowledge of the wave function allows us to analyze the photoionization dynamics and to validate the physical pictures proposed in previous experimental studies. As an outlook, we investigate how electron vortices develop from the multiphoton-to the tunnel regime with increasing laser intensity.

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“…Originally devised to describe charge-transfer processes, it was later used to illustrate features of, e.g., coupled electronic-nuclear quantum (Hader et al, 2017;Albert et al, 2017;Engel, 2019b, 2022) and classical dynamics (Schaupp and Engel, 2019a) or two-dimensional coherent femtosecond spectroscopy (Albert et al, 2015). The model was also used to study photoionisation (Falge et al, 2011(Falge et al, , 2012a(Falge et al, , 2017.…”

Section: Introductionmentioning

confidence: 99%

Nuclear–Electron Correlation Effects and Their Photoelectron Imprint in Molecular XUV Ionisation

et al. 2022

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The ionisation of molecules by attosecond XUV pulses is accompanied by complex correlated dynamics, such as the creation of coherent electron wave packets in the parent ion, their interplay with nuclear wave packets, and a correlated photoelectron moving in a multi-centred potential. Additionally, these processes are influenced by the dynamics prior to and during the ionisation. To fully understand and subsequently control the ionisation process on different time scales, a profound understanding of electron and nuclear correlation is needed. Here, we investigate the effect of nuclear–electron correlation in a correlated two-electron and one-nucleus quantum model system. Solving the time-dependent Schrödinger equation allows to monitor the correlation impact pre, during, and post-XUV ionisation. We show how an initial nuclear wave packet displaced from equilibrium influences the post-ionisation dynamics by means of momentum conservation between the target and parent ion, whilst the attosecond electron population remains largely unaffected. We calculate time-resolved photoelectron spectra and their asymmetries and demonstrate how the coupled electron–nuclear dynamics are imprinted on top of electron–electron correlation on the photoelectron properties. Finally, our findings give guidelines towards when correlation resulting effects have to be incorporated and in which instances the exact correlation treatment can be neglected.

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Time-resolved photoelectron spectroscopy of IR-driven electron dynamics in a charge transfer model system

Cited by 5 publications

References 37 publications

The impact of electron–electron correlation in ultrafast attosecond single ionization dynamics

The impact of electron–electron correlation in ultrafast attosecond single ionization dynamics

Atomic photoionization dynamics in ultrashort cycloidal laser fields

Nuclear–Electron Correlation Effects and Their Photoelectron Imprint in Molecular XUV Ionisation

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